One‐Step Transformation of Single‐Walled Carbon Nanotube Networks into High‐Performance Multilayer Graphene‐Rich Films via Laser Shockwave Compaction

Abstract An unprecedented chemical‐free, one‐step method is presented to convert single‐walled carbon nanotube (SWCNT) networks into multilayer graphene‐rich films at an exceptionally low temperature (<120 °C). This transformation is driven by high‐rate, repetitive pressure (≈2.27 GPa) from laser‐induced shockwaves, which compact and restructure the SWCNTs network to a graphenic film. A key mechanism is based on the controlled unzipping of SWCNTs under intense shockwave compaction, enabling their transition into multilayer graphene with near‐equilibrium van der Waals layer spacing. The resulting graphene‐rich films exhibit a sevenfold increase in thermal conductivity (66.25 ± 7.16 W m −1 K −1 ) and a 2.6‐fold enhancement in electrical conductivity (0.18 ± 0.06 MS m −1 ), significantly improving the thermal and electrical transport properties. This scalable and energy‐efficient method uniquely enables interface engineering and continuous sp 2 structure reconstruction, opening new avenues for high‐performance electronics, thermal management, and energy storage applications.